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VH2 is Fluorite structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. V2+ is bonded in a body-centered cubic geometry to eight equivalent H1- atoms. All V–H bond lengths are 1.83 Å. H1- is bonded to four equivalent V2+ atoms to form a mixture of corner and edge-sharing HV4 tetrahedra.
HfV2H4 crystallizes in the tetragonal I4_1/a space group. The structure is three-dimensional. Hf is bonded in a 8-coordinate geometry to eight equivalent H atoms. All Hf–H bond lengths are 2.04 Å. V is bonded in a distorted rectangular see-saw-like geometry to four equivalent H atoms. There is two shorter (1.80 Å) and two longer (1.83 Å) V–H bond length. H is bonded to two equivalent Hf and two equivalent V atoms to form a mixture of edge and corner-sharing HHf2V2 tetrahedra.